Three-dimensional strain dynamics govern the hysteresis in heterogeneous catalysis

Author(s)

Passos, Aline R. ^[1] ; Rochet, Amelie ^[1] ; Manente, Luiza M. ^[1] ; Suzana, Ana F. ^{[1, 2]} ; Harder, Ross ^[3] ; Cha, Wonsuk ^[3] ; Meneau, Florian ^[1]

Affiliation

^[1] Brazilian Ctr Res Energy & Mat CNPEM, Brazilian Synchrotron Light Lab LNLS, BR-13083970 Campinas, SP - Brazil

^[2] UNESP, Inst Quim, Rua Prof Francisco Degni, BR-14800900 Araraquara, SP - Brazil

^[3] Argonne Natl Lab, Adv Photon Source, 9700 South Cass Ave, Argonne, IL 60439 - USA

• Document type: Journal article
• Source: NATURE COMMUNICATIONS; v. 11, n. 1 SEP 18 2020.
• Web of Science Citations: 5

Abstract

Understanding catalysts strain dynamic behaviours is crucial for the development of cost-effective, efficient, stable and long-lasting catalysts. Here, we reveal in situ three-dimensional strain evolution of single gold nanocrystals during a catalytic CO oxidation reaction under operando conditions with coherent X-ray diffractive imaging. We report direct observation of anisotropic strain dynamics at the nanoscale, where identically crystallographically-oriented facets are qualitatively differently affected by strain leading to preferential active sites formation. Interestingly, the single nanoparticle elastic energy landscape, which we map with attojoule precision, depends on heating versus cooling cycles. The hysteresis observed at the single particle level is following the normal/inverse hysteresis loops of the catalytic performances. This approach opens a powerful avenue for studying, at the single particle level, catalytic nanomaterials and deactivation processes under operando conditions that will enable profound insights into nanoscale catalytic mechanisms. Direct visualisation of site-specific strain variations of catalysts is needed to better understand catalytic properties. Here, the authors determine with attojoule precision that the well-known catalytic hysteresis phenomenon occurs at single particle level and involves three-dimensional strain field. (AU)

• FAPESP's process: 14/25964-5 - From the monomers to the nanoparticles: in situ real time investigation of gold nanoparticles formation by synchrotron and microscopy techniques
• Grantee: Florian Edouard Pierre Meneau
• Support Opportunities: Research Grants - Young Investigators Grants
• FAPESP's process: 19/03162-8 - Synthesis of shaped-controlled gold nanoparticles
• Grantee: Luiza Minucci Manente
• Support Opportunities: Scholarships in Brazil - Scientific Initiation
• FAPESP's process: 14/27127-3 - Genesis of gold nanoparticles: nucleation, growth and stabilization
• Grantee: Ana Flávia Suzana
• Support Opportunities: Scholarships in Brazil - Doctorate
• FAPESP's process: 18/08816-3 - Operando coherent X-ray diffraction: imaging in 3D dimensions nanoparticle catalysts
• Grantee: Aline Ribeiro Passos
• Support Opportunities: Scholarships in Brazil - Post-Doctoral
• FAPESP's process: 17/23050-4 - Multi-modal approach probing noble-metal catalysts at work
• Grantee: Amélie Claire Rochet
• Support Opportunities: Research Grants - Young Investigators Grants